The surface chemistry of atmospheric aerosol particles is important in determining how these particles will effect human health, visibility, climate and precipitation chemistry. In previous work, it has been shown that ToF-SIMS can provide significant valuable information on both organic and inorganic constituents of the aerosol. It has been found, however, that ToF-SIMS with a Ga+ primary ion beam offers very low sensitivity to poly-aromatic hydrocarbons (PAHs) and heavy metals, two important classes of pollutants. In this work the utility of laser-SNMS for detection of these pollutants has been explored. Two laser systems, a 193 nm excimer laser and a 157 nm excimer laser have been utilized. Each approach has advantages. ToF-SIMS has the highest sensitivity to alkali metals and aliphatic hydrocarbons. The 193 nm laser provides very high sensitivity to lead and other metals. The 157 nm laser greatly enhances sensitivity to PAHs which has enabled detection of PAHs on the surface of individual particles. (c) 2006 Published by Elsevier B.V.